Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 57, Issue 49, Pages 16001-16004Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201808215
Keywords
electrocatalysis; heterogeneous catalysis; hydrogen evolution; [NiFe]-hydrogenase; reaction mechanism
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Funding
- Agence National de la Recherche [ANR-11-LABX-003, ANR-16-CE92_0012_01 NiFeMim]
- Indo-French Center for the Promotion of Advanced Research (IFCPAR/CEFIPRA grant) [5405-1]
- China Scholarship Council
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[NiFe]-hydrogenase enzymes are efficient catalysts for H-2 evolution but their synthetic models have not been reported to be active under aqueous conditions so far. Here we show that a close model of the [NiFe]-hydrogenase active site can work as a very active and stable heterogeneous H-2 evolution catalyst under mildly acidic aqueous conditions. Entry in catalysis is a (NiFeII)-Fe-I complex, with electronic structure analogous to the Ni-L state of the enzyme, corroborating the mechanism modification recently proposed for [NiFe]-hydrogenases.
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